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Charge-specific size-dependent separation of water-soluble organic molecules by fluorinated nanoporous networks.

ABSTRACT: Molecular architecture in nanoscale spaces can lead to selective chemical interactions and separation of species with similar sizes and functionality. Substrate specific sorbent chemistry is well known through highly crystalline ordered structures such as zeolites, metal organic frameworks and widely available nanoporous carbons. Size and charge-dependent separation of aqueous molecular contaminants, on the contrary, have not been adequately developed. Here we report a charge-specific size-dependent separation of water-soluble molecules through an ultra-microporous polymeric network that features fluorines as the predominant surface functional groups. Treatment of similarly sized organic molecules with and without charges shows that fluorine interacts with charges favourably. Control experiments using similarly constructed frameworks with or without fluorines verify the fluorine-cation interactions. Lack of a ?-hole for fluorine atoms is suggested to be responsible for this distinct property, and future applications of this discovery, such as desalination and mixed matrix membranes, may be expected to follow.

SUBMITTER: Byun J

PROVIDER: S-EPMC5109553 | biostudies-other | 2016 Nov

REPOSITORIES: biostudies-other

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Charge-specific size-dependent separation of water-soluble organic molecules by fluorinated nanoporous networks.

Byun Jeehye J Patel Hasmukh A HA Thirion Damien D Yavuz Cafer T CT

Nature communications 20161110

Molecular architecture in nanoscale spaces can lead to selective chemical interactions and separation of species with similar sizes and functionality. Substrate specific sorbent chemistry is well known through highly crystalline ordered structures such as zeolites, metal organic frameworks and widely available nanoporous carbons. Size and charge-dependent separation of aqueous molecular contaminants, on the contrary, have not been adequately developed. Here we report a charge-specific size-depen ...[more]

PMID: 27830697

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Project description:The chemical content of water-soluble organic carbon (WSOC) as a function of particle size was characterized in Little Rock, Arkansas in winter and spring 2013. The objectives of this study were to (i) compare the functional characteristics of coarse, fine and ultrafine WSOC and (ii) reconcile the sources of WSOC for periods when carbonaceous aerosol was the most abundant particulate component. The WSOC accounted for 5 % of particle mass for particles with ?p > 0.96 ?m and 10 % of particle mass for particles with ?p < 0.96 ?m. Non-exchangeable aliphatic (H-C), unsaturated aliphatic (H-C-C=), oxygenated saturated aliphatic (H-C-O), acetalic (O-CH-O) and aromatic (Ar-H) protons were determined by proton nuclear magnetic resonance ((1)H-NMR). The total non-exchangeable organic hydrogen concentrations varied from 4.1 ± 0.1 nmol m(-3) for particles with 1.5 < ?p < 3.0 ?m to 73.9 ± 12.3 nmol m(-3) for particles with ?p < 0.49 ?m. The molar H/C ratios varied from 0.48 ± 0.05 to 0.92 ± 0.09, which were comparable to those observed for combustion-related organic aerosol. The R-H was the most abundant group, representing about 45 % of measured total non-exchangeable organic hydrogen concentrations, followed by H-C-O (27 %) and H-C-C= (26 %). Levoglucosan, amines, ammonium and methanesulfonate were identified in NMR fingerprints of fine particles. Sucrose, fructose, glucose, formate and acetate were associated with coarse particles. These qualitative differences of (1)H-NMR profiles for different particle sizes indicated the possible contribution of biological aerosols and a mixture of aliphatic and oxygenated compounds from biomass burning and traffic exhausts. The concurrent presence of ammonium and amines also suggested the presence of ammonium/aminium nitrate and sulfate secondary aerosol. The size-dependent origin of WSOC was further corroborated by the increasing ?(13)C abundance from -26.81 ± 0.18 ‰ for the smallest particles to -25.93 ± 0.31 ‰ for the largest particles and the relative distribution of the functional groups as compared to those previously observed for marine, biomass burning and secondary organic aerosol. The latter also allowed for the differentiation of urban combustion-related aerosol and biological particles. The five types of organic hydrogen accounted for the majority of WSOC for particles with ?p > 3.0 ?m and ?p < 0.96 ?m.

Dataset Information

Charge-specific size-dependent separation of water-soluble organic molecules by fluorinated nanoporous networks.

Publications

Charge-specific size-dependent separation of water-soluble organic molecules by fluorinated nanoporous networks.

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